ABSTRACT
Heavy-fermion metals are prototype systems for observing emergent quantum phases driven by electronic interactions1-6. A long-standing aspiration is the dimensional reduction of these materials to exert control over their quantum phases7-11, which remains a significant challenge because traditional intermetallic heavy-fermion compounds have three-dimensional atomic and electronic structures. Here we report comprehensive thermodynamic and spectroscopic evidence of an antiferromagnetically ordered heavy-fermion ground state in CeSiI, an intermetallic comprising two-dimensional (2D) metallic sheets held together by weak interlayer van der Waals (vdW) interactions. Owing to its vdW nature, CeSiI has a quasi-2D electronic structure, and we can control its physical dimension through exfoliation. The emergence of coherent hybridization of f and conduction electrons at low temperature is supported by the temperature evolution of angle-resolved photoemission and scanning tunnelling spectra near the Fermi level and by heat capacity measurements. Electrical transport measurements on few-layer flakes reveal heavy-fermion behaviour and magnetic order down to the ultra-thin regime. Our work establishes CeSiI and related materials as a unique platform for studying dimensionally confined heavy fermions in bulk crystals and employing 2D device fabrication techniques and vdW heterostructures12 to manipulate the interplay between Kondo screening, magnetic order and proximity effects.
ABSTRACT
Electronic flat-band materials host quantum states characterized by a quenched kinetic energy. These flat bands are often conducive to enhanced electron correlation effects and emergent quantum phases of matter1. Long studied in theoretical models2-4, these systems have received renewed interest after their experimental realization in van der Waals heterostructures5,6 and quasi-two-dimensional (2D) crystalline materials7,8. An outstanding experimental question is if such flat bands can be realized in three-dimensional (3D) networks, potentially enabling new materials platforms9,10 and phenomena11-13. Here we investigate the C15 Laves phase metal CaNi2, which contains a nickel pyrochlore lattice predicted at a model network level to host a doubly-degenerate, topological flat band arising from 3D destructive interference of electronic hopping14,15. Using angle-resolved photoemission spectroscopy, we observe a band with vanishing dispersion across the full 3D Brillouin zone that we identify with the pyrochlore flat band as well as two additional flat bands that we show arise from multi-orbital interference of Ni d-electrons. Furthermore, we demonstrate chemical tuning of the flat-band manifold to the Fermi level that coincides with enhanced electronic correlations and the appearance of superconductivity. Extending the notion of intrinsic band flatness from 2D to 3D, this provides a potential pathway to correlated behaviour predicted for higher-dimensional flat-band systems ranging from tunable topological15 to fractionalized phases16.
ABSTRACT
A variety of 'strange metals' exhibit resistivity that decreases linearly with temperature as the temperature decreases to zero1-3, in contrast to conventional metals where resistivity decreases quadratically with temperature. This linear-in-temperature resistivity has been attributed to charge carriers scattering at a rate given by h/τ = αkBT, where α is a constant of order unity, h is the Planck constant and kB is the Boltzmann constant. This simple relationship between the scattering rate and temperature is observed across a wide variety of materials, suggesting a fundamental upper limit on scattering-the 'Planckian limit'4,5-but little is known about the underlying origins of this limit. Here we report a measurement of the angle-dependent magnetoresistance of La1.6-xNd0.4SrxCuO4-a hole-doped cuprate that shows linear-in-temperature resistivity down to the lowest measured temperatures6. The angle-dependent magnetoresistance shows a well defined Fermi surface that agrees quantitatively with angle-resolved photoemission spectroscopy measurements7 and reveals a linear-in-temperature scattering rate that saturates at the Planckian limit, namely α = 1.2 ± 0.4. Remarkably, we find that this Planckian scattering rate is isotropic, that is, it is independent of direction, in contrast to expectations from 'hotspot' models8,9. Our findings suggest that linear-in-temperature resistivity in strange metals emerges from a momentum-independent inelastic scattering rate that reaches the Planckian limit.
ABSTRACT
BACKGROUND: ß-aminopropionitrile (BAPN) is a pharmacological inhibitor of LOX (lysyl oxidase) and LOXLs (LOX-like proteins). Administration of BAPN promotes aortopathies, although there is a paucity of data on experimental conditions to generate pathology. The objective of this study was to define experimental parameters and determine whether equivalent or variable aortopathies were generated throughout the aortic tree during BAPN administration in mice. METHODS: BAPN was administered in drinking water for a period ranging from 1 to 12 weeks. The impacts of BAPN were first assessed with regard to BAPN dose, and mouse strain, age, and sex. BAPN-induced aortic pathological characterization was conducted using histology and immunostaining. To investigate the mechanistic basis of regional heterogeneity, the ascending and descending thoracic aortas were harvested after 1 week of BAPN administration before the appearance of overt pathology. RESULTS: BAPN-induced aortic rupture predominantly occurred or originated in the descending thoracic aorta in young C57BL/6J or N mice. No apparent differences were found between male and female mice. For mice surviving 12 weeks of BAPN administration, profound dilatation was consistently observed in the ascending region, while there were more heterogeneous changes in the descending thoracic region. Pathological features were distinct between the ascending and descending thoracic regions. Aortic pathology in the ascending region was characterized by luminal dilatation and elastic fiber disruption throughout the media. The descending thoracic region frequently had dissections with false lumen formation, collagen deposition, and remodeling of the wall surrounding the false lumen. Cells surrounding the false lumen were predominantly positive for α-SMA (α-smooth muscle actin). One week of BAPN administration compromised contractile properties in both regions equivalently, and RNA sequencing did not show obvious differences between the 2 aortic regions in smooth muscle cell markers, cell proliferation markers, and extracellular components. CONCLUSIONS: BAPN-induced pathologies show distinct, heterogeneous features within and between ascending and descending aortic regions in mice.
Subject(s)
Aminopropionitrile , Aorta, Thoracic , Aortic Rupture , Disease Models, Animal , Mice, Inbred C57BL , Animals , Aminopropionitrile/toxicity , Aminopropionitrile/pharmacology , Aorta, Thoracic/pathology , Aorta, Thoracic/drug effects , Aorta, Thoracic/metabolism , Female , Male , Aortic Rupture/chemically induced , Aortic Rupture/pathology , Aortic Rupture/metabolism , Aortic Rupture/prevention & control , Mice , Vascular Remodeling/drug effects , Dilatation, Pathologic , Muscle, Smooth, Vascular/pathology , Muscle, Smooth, Vascular/drug effects , Muscle, Smooth, Vascular/metabolism , Age Factors , Time Factors , Sex Factors , Cell Proliferation/drug effects , Protein-Lysine 6-Oxidase/metabolismABSTRACT
Heterostructures can be assembled from atomically thin materials by combining a wide range of available van der Waals crystals, providing exciting possibilities for designer electronics 1 . In many cases, beyond simply realizing new material combinations, interlayer interactions lead to emergent electronic properties that are fundamentally distinct from those of the constituent layers 2 . A critical parameter in these structures is the interlayer coupling strength, but this is often not easy to determine and is typically considered to be a fixed property of the system. Here we demonstrate that we can controllably tune the interlayer separation in van der Waals heterostructures using hydrostatic pressure, providing a dynamic way to modify their electronic properties. In devices in which graphene is encapsulated in boron nitride and aligned with one of the encapsulating layers, we observe that increasing pressure produces a superlinear increase in the moiré-superlattice-induced bandgap-nearly doubling within the studied range-together with an increase in the capacitive gate coupling to the active channel by as much as 25 per cent. Comparison to theoretical modelling highlights the role of atomic-scale structural deformations and how this can be altered with pressure. Our results demonstrate that combining hydrostatic pressure with controlled rotational order provides opportunities for dynamic band-structure engineering in van der Waals heterostructures.
ABSTRACT
The kagome metals display an intriguing variety of electronic and magnetic phases arising from the connectivity of atoms on a kagome lattice. A growing number of these materials with vanadium-kagome nets host charge-density waves (CDWs) at low temperatures, including ScV6Sn6, CsV3Sb5, and V3Sb2. Curiously, only the Sc version of the RV6Sn6 materials with a HfFe6Ge6-type structure hosts a CDW (R = Gd-Lu, Y, Sc). In this study, we investigate the role of rare earth size in CDW formation in the RV6Sn6 compounds. Magnetization measurements on our single crystals of (Sc,Lu)V6Sn6 and (Sc,Y)V6Sn6 establish that the CDW is suppressed by substituting Sc by larger Lu or Y. Single-crystal X-ray diffraction reveals that compressible Sn-Sn bonds accommodate the larger rare earth atoms within loosely packed R-Sn-Sn chains without significantly expanding the lattice. We propose that Sc provides extra room in these chains crucial to CDW formation in ScV6Sn6. Our rattling chain model explains why both physical pressure and substitution by larger rare earth atoms hinder CDW formation despite opposite impacts on lattice size. We emphasize the cooperative effect of pressure and rare earth size by demonstrating that pressure further suppresses the CDW in a Lu-doped ScV6Sn6 crystal. Our model not only addresses why a CDW only forms in the RV6Sn6 materials with tiny Sc but also advances our understanding of why unusual CDWs form in the kagome metals.
ABSTRACT
Spin triplet superconductor UTe_{2} is widely believed to host a quasi-two-dimensional Fermi surface, revealed by first-principles calculations, photoemission, and quantum oscillation measurements. An outstanding question still remains as to the existence of a three-dimensional Fermi surface pocket, which is crucial for our understanding of the exotic superconducting and topological properties of UTe_{2}. This 3D Fermi surface pocket appears in various theoretical models with different physics origins, but has not been unambiguously detected in experiment. Here for the first time we provide concrete evidence for a relatively isotropic, small Fermi surface pocket of UTe_{2} via quantum oscillation measurements. In addition, we observed high frequency quantum oscillations corresponding to electron-hole tunneling between adjacent electron and hole pockets. The coexistence of 2D and 3D Fermi surface pockets, as well as the breakdown orbits, provide a test bed for theoretical models and aid the realization of a unified understanding of the superconducting state of UTe_{2} from the first-principles approach.
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PURPOSE: The influence of lateral patellofemoral osteoarthritis (PFOA) in medial unicompartmental knee arthroplasty (UKA) is controversial. Our aim was to identify radiographic factors that may lead to progressive PFOA after implantation of a fixed-bearing medial UKA and their impact on patient-reported outcomes (PROMs). METHODS: A retrospective consecutive cohort of patients undergoing medial UKA with a minimum follow-up of 60 months between September 2011 and January 2017 was identified. All UKAs had a fixed-bearing design with cemented femoral and tibial components. PROMs included documentation of the Oxford Knee Score (OKS). The following radiographic parameters were evaluated on conventional radiographs and computer tomography (CT) scans: patella tilt angle, patella congruence angle, Caton-Deschamps index, medial and lateral patellofemoral degeneration (Kellgren-Lawrence Classification (KL)), mechanical anteroposterior axis, femoral torsion, tibial tuberosity to trochlear groove distance (TTTG), anteroposterior translation of the femoral component. A hierarchical multiple regression analysis and partial Pearson correlation analysis (SPSS) were used to evaluate for predictors of progression of lateral PFOA. RESULTS: Forty-nine knees allowed PFOA assessment and had an average follow-up of 62 months (range 60-108). Twenty-three patients did not exhibit any progression of lateral PFOA. Twenty-two progressed with 1 stage, whereas four had progressed 2 stages according to the KL classification. TTTG negatively correlated with progressive lateral PFOA (r = - 0.436, p = 0.01). Progression of lateral PFOA did not correlate with OKS at last follow-up (p = 0.613). CONCLUSION: A decreased TTGT correlated with radiographic progression of lateral PFOA after medial fixed-bearing cemented UKA. PFOA however did not influence PROMs at a minimum of five years postoperatively.
Subject(s)
Arthroplasty, Replacement, Knee , Bone Diseases , Knee Prosthesis , Osteoarthritis, Knee , Patellofemoral Joint , Humans , Arthroplasty, Replacement, Knee/adverse effects , Arthroplasty, Replacement, Knee/methods , Patellofemoral Joint/diagnostic imaging , Patellofemoral Joint/surgery , Follow-Up Studies , Retrospective Studies , Treatment Outcome , Osteoarthritis, Knee/diagnostic imaging , Osteoarthritis, Knee/surgery , Knee Joint/diagnostic imaging , Knee Joint/surgery , Bone Diseases/surgeryABSTRACT
PURPOSE: To analyze the outcome of surgical treatment of tarsal coalition, assess the role of the surgical technique, as well as of coalition size and type on outcomes. METHODS: The search followed the Preferred Reporting Items of Systematic Review and Meta-Analysis and was performed in four databases: MEDLINE, Central, Scopus and Web of Science. The protocol has been registered in the international prospective register of systematic reviews. Patient-reported outcomes (PROMs), complications, revisions and radiographic recurrence were collected. Risk of bias was assessed using MINORS criteria. A random-effects model for meta-analysis was applied for analysis of data heterogeneity. RESULTS: Twenty-five studies including 760 tarsal coalitions were included and had a weighted average follow-up of 44 months. Studies scored fair to poor on the risk of bias assessment with a mean MINORS score of 67% (44-81%). In 77.8% (37.5-100%) of surgically treated tarsal coalitions, good/excellent/non-limiting or improved PROMs were reported. Calculated data heterogeneity was moderate (I2 = 57%). Open bar resection with material interposition had a clinical success rate of 78.8% (50-100%). Complications occurred in 4.96% of cases. Coalition size did not prove to be a determining factor in postoperative outcome. The influence of the coalition type was not investigated by any of the studies. CONCLUSION: Data on outcomes of surgical management for tarsal coalitions is limited to retrospective case series with high risk of bias and moderate data heterogeneity. In about ¾ of cases, open resection and interposition of material results in improved PROMs. The arbitrary margin of ≥ 50% of TC coalition size in relation to the posterior facet has little importance in surgical decision-making. None of the studies reported on the influence of the coalition type on postoperative clinical success.
Subject(s)
Synostosis , Tarsal Bones , Tarsal Coalition , Humans , Retrospective Studies , Synostosis/complications , Synostosis/surgery , Systematic Reviews as Topic , Tarsal Bones/surgery , Tarsal Coalition/complicationsABSTRACT
Emergent relativistic quasiparticles in Weyl semimetals are the source of exotic electronic properties such as surface Fermi arcs, the anomalous Hall effect and negative magnetoresistance, all observed in real materials. Whereas these phenomena highlight the effect of Weyl fermions on the electronic transport properties, less is known about what collective phenomena they may support. Here, we report a Weyl semimetal, NdAlSi, that offers an example. Using neutron diffraction, we found a long-wavelength helical magnetic order in NdAlSi, the periodicity of which is linked to the nesting vector between two topologically non-trivial Fermi pockets, which we characterize using density functional theory and quantum oscillation measurements. We further show the chiral transverse component of the spin structure is promoted by bond-oriented Dzyaloshinskii-Moriya interactions associated with Weyl exchange processes. Our work provides a rare example of Weyl fermions driving collective magnetism.
ABSTRACT
The connection between unconventional superconductivity and charge density waves (CDWs) has intrigued the condensed matter community and found much interest in the recently discovered superconducting Kagome family of AV_{3}Sb_{5} (A=K, Cs, Rb). X-ray diffraction and Raman spectroscopy measurements established that the CDW order in CsV_{3}Sb_{5} comprises of a 2×2×4 structure with stacking of layers in a star-of-David (SD) and inverse-star-of-David (ISD) pattern along the c-axis direction. Such interlayer ordering will induce a vast normalization of the electronic ground state; however, it has not been observed in Fermi surface measurements. Here we report quantum oscillations of CsV_{3}Sb_{5} using tunnel diode oscillator frequency measurements. We observed a large number of frequencies, many of which were not reported. The number of frequencies cannot be explained by DFT calculations when only SD or ISD distortion is considered. Instead, our results are consistent with calculations when interlayer ordering is taken into account, providing strong evidence that the CDW phase of CsV_{3}Sb_{5} has complicated structure distortion which in turn has dramatic effects on the Fermi surface properties.
ABSTRACT
In a topological semimetal with Dirac or Weyl points, the bulk-boundary correspondence principle predicts a gapless edge mode if the essential symmetry is still preserved at the surface. The detection of such topological surface state has been considered as the fingerprint prove for crystals with nontrivial topological bulk band. On the contrary, it has been proposed that even with symmetry broken at the surface, a new surface band can emerge in nonsymmorphic topological semimetals. The symmetry reduction at the surface lifts the bulk band degeneracies and produces an unusual "floating" surface band with trivial topology. Here, we first report quantum transport probing to ZrSiSe thin flakes and directly reveal transport signatures of this new surface state. Remarkably, though topologically trivial, such a surface band exhibits substantial two-dimensional Shubnikov-de Haas quantum oscillations with high mobility, which signifies a new protection mechanism and may open applications for quantum computing and spintronic devices.
ABSTRACT
A kagome lattice of 3d transition metal ions is a versatile platform for correlated topological phases hosting symmetry-protected electronic excitations and magnetic ground states. However, the paradigmatic states of the idealized two-dimensional kagome lattice-Dirac fermions and flat bands-have not been simultaneously observed. Here, we use angle-resolved photoemission spectroscopy and de Haas-van Alphen quantum oscillations to reveal coexisting surface and bulk Dirac fermions as well as flat bands in the antiferromagnetic kagome metal FeSn, which has spatially decoupled kagome planes. Our band structure calculations and matrix element simulations demonstrate that the bulk Dirac bands arise from in-plane localized Fe-3d orbitals, and evidence that the coexisting Dirac surface state realizes a rare example of fully spin-polarized two-dimensional Dirac fermions due to spin-layer locking in FeSn. The prospect to harness these prototypical excitations in a kagome lattice is a frontier of great promise at the confluence of topology, magnetism and strongly correlated physics.
ABSTRACT
In the vicinity of a quantum critical point, quenched disorder can lead to a quantum Griffiths phase, accompanied by an exotic power-law scaling with a continuously varying dynamical exponent that diverges in the zero-temperature limit. Here, we investigate a nematic quantum critical point in the iron-based superconductor FeSe_{0.89}S_{0.11} using applied hydrostatic pressure. We report an unusual crossing of the magnetoresistivity isotherms in the nonsuperconducting normal state that features a continuously varying dynamical exponent over a large temperature range. We interpret our results in terms of a quantum Griffiths phase caused by nematic islands that result from the local distribution of Se and S atoms. At low temperatures, the Griffiths phase is masked by the emergence of a Fermi liquid phase due to a strong nematoelastic coupling and a Lifshitz transition that changes the topology of the Fermi surface.
ABSTRACT
Chemical vapor deposition (CVD) of UO2 thin films from in situ reductive decomposition using a U(VI) precursor ([U(OtBu)6]) was performed under applied magnetic fields (up to 1 T). The molecular mechanism responsible for the formation of U(IV) oxide was determined by nuclear magnetic resonance (NMR) analysis of gaseous byproducts revealed a reductive transformation of uranium hexakis-tert-butoxide into urania. Thin films were grown under zero-field and applied magnetic field conditions that clearly showed the guiding influence of the magnetic field on altering the morphology and crystallographic orientation of grains in UO2 deposits produced under an external magnetic field. Application of magnetic fields was found to reduce the grain size. Whereas films with a ⟨111⟩ preferred orientation were observed under zero-field conditions, the application of magnetic fields (500 mT to 1 T) promoted a polycrystalline growth. X-ray photoelectron spectroscopy confirmed the formation of UO2 films with traces of U(VI) centers present on the surface, which was evidently due to the surface oxidation of coordinatively unsaturated U(IV) centers, which was found to be significantly reduced in the field-assisted process. These findings emphasize the positive effect of magnetic fields on controlling the texture and chemical homogeneity of CVD-grown films. The availability of a magnetic field as an extrinsic parameter for the CVD process adds to the conventional parameters, such as temperature, deposition time, and pressure, and expands the experimental space for thin-film growth.
ABSTRACT
The physical properties of two-dimensional van der Waals crystals can be sensitive to interlayer coupling. For two-dimensional magnets1-3, theory suggests that interlayer exchange coupling is strongly dependent on layer separation while the stacking arrangement can even change the sign of the interlayer magnetic exchange, thus drastically modifying the ground state4-10. Here, we demonstrate pressure tuning of magnetic order in the two-dimensional magnet CrI3. We probe the magnetic states using tunnelling8,11-13 and scanning magnetic circular dichroism microscopy measurements2. We find that interlayer magnetic coupling can be more than doubled by hydrostatic pressure. In bilayer CrI3, pressure induces a transition from layered antiferromagnetic to ferromagnetic phase. In trilayer CrI3, pressure can create coexisting domains of three phases, one ferromagnetic and two antiferromagnetic. The observed changes in magnetic order can be explained by changes in the stacking arrangement. Such coupling between stacking order and magnetism provides ample opportunities for designer magnetic phases and functionalities.
ABSTRACT
Electrical transport measurements were performed on URu2 - x Fe x Si2 single-crystal specimens in high magnetic fields up to 45 T (DC fields) and 60 T (pulsed fields). We observed a systematic evolution of the critical fields for both the hidden-order (HO) and large-moment antiferromagnetic (LMAFM) phases and established the 3D phase diagram of T-H-x In the HO phase, H/H0 scales with T/T0 and collapses onto a single curve. However, in the LMAFM phase, this single scaling relation is not satisfied. Within a certain range of x values, the HO phase reenters after the LMAFM phase is suppressed by the magnetic field, similar to the behavior observed for URu2Si2 within a certain range of pressures.
ABSTRACT
New heteroleptic rhenium(I) compounds, [fac-Re(I)(CO)3(L)] (e.g., L= tfb-dmpda, (N,N-(4,4,4-trifluorobut-1-en-3-on)-dimethyl propylene diamine)), containing anionic and neutral ligands act as efficient precursors to grow polycrystalline rhenium nitride (ReN) films by their vapor phase deposition at 600 °C. Deposition of ReN films under an external magnetic field showed an orientation effect with preferred growth of crystallites along ⟨100⟩ direction. Rhenium complexes reported here unify high stability and reactivity in a single molecule through a Janus-type coordination around a Re center, constituted by a chelating tridentate ligand and three carbonyl groups imparting a facial geometry. Single-crystal diffraction analysis confirmed the structural integrity of the new rhenium compounds. The rigidity of molecular framework was validated in solution via 1D and 2D NMR spectroscopy, in the gas phase via mass spectrometry, and in the solid-state by thermogravimetric analysis and differential scanning calorimetry studies. The analytical data showed that pre-existent Re-N bonds in [fac-Re(I)(CO)3(L)] facilitated low-temperature formation of crystalline ReN deposits confirmed by grazing angle X-ray diffraction analysis. The surface chemical composition and the uniformity of microstructure were provided by X-ray photoelectron spectroscopy (XPS) and scanning and transmission electron microscopy (SEM/TEM), respectively.
ABSTRACT
The simple system of tetraammonium octafluorouranate is employed to derive a fundamental understanding of the uranium-fluorine interaction. The structure is composed of isolated molecules, enabling a detailed examination of the U4+ ( f2) ion. Characterization of single-crystals by X-ray diffraction, absorption spectroscopy, and magnetic analysis up to 45 T is combined with extensive theoretical treatment by CASSCF. The influence of different active spaces and representations of the structure is examined in the context of the experimental evidence. The Interacting Quantum Atoms method (IQA) is used to examine the nature of the U-F bond, concluding that there is a non-negligible degree of covalent character (9% of the total bond energy) in [UF8]4-. For the structural and theoretical reasons discussed herein, it is proposed that the structure of (NH4)4UF8 may be appropriately employed as a benchmark compound for future theoretical characterization of U(IV).
ABSTRACT
Quasiparticles with Dirac-type dispersion can be observed in nearly gapless bulk semiconductors alloys in which the bandgap is controlled through the material composition. We demonstrate that the Dirac dispersion can be realized in short-period InAs1-xSbx/InAs1-ySby metamorphic superlattices with the bandgap tuned to zero by adjusting the superlattice period and layer strain. The new material has anisotropic carrier dispersion: the carrier energy associated with the in-plane motion is proportional to the wave vector and characterized by the Fermi velocity vF, and the dispersion corresponding to the motion in the growth direction is quadratic. Experimental estimate of the Fermi velocity gives vF = 6.7 × 105 m/s. Remarkably, the Fermi velocity in this system can be controlled by varying the overlap between electron and hole states in the superlattice. Extreme design flexibility makes the short-period metamorphic InAs1-xSbx/InAs1-ySby superlattice a new prospective platform for studying the effects of charge-carrier chirality and topologically nontrivial states in structures with the inverted bandgaps.